Polaire went on to act in the theatre. Her first major appearance was in 1902, at the Théâtre des Bouffes Parisiens, in the title role of a play based on Colette's Claudine à Paris. A gifted comedic actress, she became one of the major celebrities of her day.

At a time when tightlacing among women was in vogue, she was famous for her tiny, corsetted waist, which was sometimes reported to have a circumference no greater than 14 inches (35.6 centimeters). This accentuated her large bust, which was said to measure 38 inches (96.5 centimeters). She stood 5 feet and 3 inches (1.60 meters) tall. Talk of her figure and her lavish overdressing in fur coats and dazzling jewels preceded her appearances wherever she went. Jean Lorrain said of her

Polaire! The agitating and agitated Polaire! The tiny slip of a woman that you know, with the waist slender to the point of pain, of screaming out loud, of breaking in two, in a spasmically tight bodice, the prettiest slimness ... And, under the aureole of an extravagant masher's hat, orange and plumed with iris leaves, the great voracious mouth, the immense black eyes, ringed, bruised, discoloured, the incandescence of her pupils, the bewildered nocturnal hair, the phosphorus, the sulphur, the red pepper of that ghoulish, Salome-like face, the agitating and agitated Polaire!What a devilish mimic, what a coffee-mill and what a belly-dancer! Yellow skirt tucked high, gloved in open-work stockings, Polaire skips, flutters, wriggles, arches from the hips, the back, the belly, mimes every kind of shock, twists, coils, rears, twirls...trembling like a stuck wasp, miaows, faints to what music and what words! The house, frozen with stupor, forgets to applaud.

In 1911, as Pauline Polaire, she was cast her in her first silent-film role. In the next year, she was offered a role in a film by the up-and-coming young director Maurice Tourneur; she appeared in six of his films in 1912 and 1913. She then returned to the musical stage and began a tour of the United States, after which she appeared at the LondonColiseum. Polaire returned to films in 1922; she performed in ten between then and 1935, some of them talkies.

She died in 1939, at age sixty-five; her body was buried at the Cimetière du Centre, in the eastern Paris suburb of Champigny-sur-Marne.